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Removal of Uranium and Molybdenum From 0J.-9. REMOVAL OF URANIUM AND MOLYBDENUM FROM URANIUM MINE WASTEWATERS BY ALGAE by Katherine T. Dreher Submitted in Partial Fulfillment of the Requirements for the Degree of Master of Chemistry New Mexico Institute of Mining and Technology Socorro, New M1exico lo)'3 9308180134 93080511 December, 1980 PDR WASTE WM-11 PDR TABLE OF CONTENTS Page Acknowledgements ........................................ ii Abstract ................................................ iii List of Tables .......................................... v List of Figures ......................................... vi I. INTRODUCTION ...................................... 1 A. Bioaccumulation of Heavy Metals ............. 1 B. Mechanisms of Uptake of Heavy Metals ........ 3 C. Algae, Metal and Sediment Interactions ...... 7 D. Objectives of Present Study ................. 9 II. MATERIALS AND METHODS ................ 10 A. Site Description ............... 10 B. Collection Procedure ........... 14 C. Laboratory Culture ............. 14 D. Algae Digestions ............... 14 E. Uranium Toxicity Test .......... 17 F. 24-Hour Uptake of Molybdenum and Uranium.................... S............. 18 G. Long-Term Studies .............. S.... ......... 2 1 H. Analytical Procedures .......... S............. 23 I. SEM Studies .................... ............. 23 III. RESULTS .............................. S............. 25 A. Algae Populations .............. S............. 25 B. Laboratory Culture ............. 26 C. Metal Levels in Field-Collected Algae....... 30 D. Uranium Toxicity ............... 0 34 " 0 E. 24-Hour Uptake ................. 37 F. Long-Term Uptake ............... i 41 IV. DISCUSSION ........................................ 54 APPENDIX A. Analytical Procedures ................ 63 APPENDIX B. Statistical Test Values .............. 66 REFERENCES ........................................ 68 Sii ACKNOWLEDGEMENTS My foremost thanks go to my adviser, Dr. James Brierley, for his patient, continued encouragement of this work and for his many suggestions for lines of research and methods for carrying them out. I thank my committee members, Corale Brierley and Dr. Donald Brandvold, for their help ful discussions and for their interest in the research. Dr. Thomas Lynch's help with the pond productivity calcu lations and with the statistical methods is greatly appreciated. My special thanks go to Barbara Popp, John Hagstrom and J. D. Murray, at the New Mexico Bureau of Mines and Mineral Resources, for meticulously performing so many of the quantitative analyses. James Cleveland, Chief Environmentalist for the Kerr McGee Corporation, provided the opportunity to sample the treatment pond system. This work was supported by the New Mexico Water Resources Research Center grant 1345639 and by the United States Bureau of Mines contract #J0295033, subcontracted from the Center for Environmental Sciences, University of Colorado at Denver, directed by Dr. Willard R. Chappell. ii i ABSTRACT Uranium mine wastewaters at the Kerr McGee Corporation site near Grants, New Mexico, are treated in part by retention in a series of ponds which support a mixed bacterial and algal flora. The pond algae, predominately Chara, Spirogyra, and Oscillatoria, accumulate uranium and molybdenum from minewater. In Chara, average levels were 440-580 ppm uranium and 0-22 ppm molybdenum. Levels in filamentous algae varied over the year from 1090-24?0 ppm uranium and 29-260 ppm molybdenum; the lower values were observed in summer and the higher in winter. In labora tory studies, Spirogyra removed more uranium and molybde num from solution than Chara in 24-hour uptake. Grinding Spirogyra cells increased removal of uranium and molybde num 2- to 3-fold over whole cells, with up to 82" removal of uranium and 37' removal of molybdenum. In long-term studies involving decaying algae in contact with sediment, the addition of algae to sediment promoted reducing conditions and usually increased sediment retention of uranium and molybdenum, but removal was reversible unless the model system contained high levels of organic material and sediment. In the present algae pond system, the mass of algae is insufficient. 4o remove significant levels of uranium and molybdenum from the high volume of minewater. .1\V Increasing pond productivity would not produce enough algae to reduce the present levels of uraniurm and molybdenum by algal adsorption alone. However, greater productivity might enhance removal by increasing the amount of organic substrate available for sulfate-reducing bacteria, thus promoting hydrogen sulfide production in pond sediments, which would enhance trace contaminant removal. LIST OF TABLES Table Page I. Chemical Parameters in Pond Water and Sediment .......................................... 12 II. Media Used in Laboratory Culture of Algae ...... 15 III. Conditions of 24-Hour Experiments .............. 20 IV. Conditions of Long-Term Experiments ............ 22 V. Test for Recovery of Uranium and Molybdenum in Digestion of Algae ................ 31 VI. Uranium and Molybdenum Levels in Field-Collected Algae ............................ 32 VII. Uranium and Molybdenum Levels in Field Collected Algae Averaged over Ponds 1, 2 and 3 ........................................ 33 VIII. Growth of Algae in Increasing Concentrations of Uranium ........................ 35 IX. 24-Hour Uptake of Molybdenum and Uranium by Chara and Spirogyra. ......................... 39 X. Long-Term Experiment I: Uptake of Uranium and Molybdenum by Spirogyra ............ 43 XI. Long-Term Experiment II: Uptake of Uranium and Molybdenum by Chara in Presence of Sediment ......................... 45 XII. Long-Term Experiment III: Uptake of Uranium and Molybdenum by Chara and Spirogyra in Presence of Sediment .......... 48 XIII. Long-Term Experiment IV: Uptake of Uranium and Molybdenum by Chara and Sediment in Dark-Maintained Cultures ....... 51 XIV. Eh Measurements for Long-Term Experiment IV Chara and Sediment in Dark-Maintained Culture.. 53 XV. Long-Term Experiment IV: Percentage of Uranium and Molybdenum Removed by Chara and Sediment in Dark-Mainained Culture ........... 53 vi LIST OF FIGURES Figure Page 1. Schematic Representation of Pond System ........ 11 2. Chara. SEM micrograph ........................... 27 3. Spirogyra. SEM micrograph ...................... 28 4. Oscillatoria. SEM micrograph ................... 29 I. INTRODUCTION A. Bioaccumulation of Heavy Metals Wastewaters from industrial and mining operations often contain heavy metal pollutants in quantities too small to warrant recovery by conventional extractive techniques, but which must be removed to maintain water quality stand ards. Uranium minewaters, for example, may contain dilute concentrations of uranium, molybdenum, selenium, radium, and other associated ions (Brierley and Brierley, 1980). Lead mines discharge waters with low levels of lead, zinc, copper, cadmium and manganese (Gale and Wixson, 1979), and the zinc industry discharges zinc, cadmium, copper, and mercury in its effluents (Jackson, 1978). The possibility of using algae for water treatment has been considered as a low-cost alternative for removing such mixtures of metals, as the ability of algae to accumulate a range of heavy metals has been recognized (Jennett, Iassett, and Smith, 1979). The bioaccumulation of heavy metals by microorganisms has been investigated extensively in relation to environ mental pollution (Gadd and Griffiths, 1978; Leland et al., 1978). Analyses of algae collected in contaminated waters show concentrations of metals 102 to 104 times higher than in surrounding waters (McDuffy et al., 1976; Ray and White, 1976; Trollope and Evans, 1976). Good correlations between concentrations of copper and lead in seawater and benthic algae were found by Seeliger and Edwards (1977), who suggested that algae might be used as indicators of environmental pollution. However, changes in the density and structure of naturally fluctuating populations, as well as physical and chemical differences in algal species, often obscure the relationship between concentrations in solution and concentrations in algae (Briand, Trucco, and Ramamoorthy, 1978; Knauer and Martin, 1973). Canterford, Buchanan and Ducker (1978) reported that concentrations of zinc, cadmium and lead in a marine diatom increased with higher external concentrations, but that the percentage of metals removed from water decreased at the higher concentrations. Coleman, Coleman and Rice (1971), using concentrations of up to 35 ppm zinc and 3 ppm cobalt, reported increased percentage uptake by freshwater algae with increasing concentrations of metals. The study of microbial bioaccumulation in respect to treatment of polluted waters has been given increasing attention (Kelly, Norris and Brierley, 1979). Several water treatment systems have been developed to take advantage of the metal concentrating ability of algae. Gale and Wixson (1979) have investigated an artificial stream meander system which has beon successful in remov ing lead, zinc and copper from lead mine effluents. Evidence indicated that the mixed algal flora, including Cladophora, Rhizoclonium, IHydrodictyon, and Spirogyra, entrapped suspended mineral particles and accumulated metals by a cation exchange process. Investigation of zinc mine and smelter wastewaters by Jackson (197S) showed that planktonic algae blooms, stimulated by sewage effluents, removed zinc and some cadmium and copper from solution. A system of sequential ponds was suggested to maximize contact with the
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